We report on a systematic study of optical properties of (Ga,Mn)As epilayers spanning the wide range of accessible substitutional Mn_Ga dopings. The growth and post-growth annealing procedures were optimized for each nominal Mn doping in order to obt
ain films which are as close as possible to uniform uncompensated (Ga,Mn)As mixed crystals. We observe a broad maximum in the mid-infrared absorption spectra whose position exhibits a prevailing blue-shift for increasing Mn-doping. In the visible range, a peak in the magnetic circular dichroism blue shifts with increasing Mn-doping. These observed trends confirm that disorder-broadened valence band states provide a better one-particle representation for the electronic structure of high-doped (Ga,Mn)As with metallic conduction than an energy spectrum assuming the Fermi level pinned in a narrow impurity band.
After decades of research, the low Curie temperature of ferromagnetic semiconductors remains the key problem in the development of magnetic semiconductor spintronic technologies. Removing this roadblock might require a change of the fields basic mate
rials paradigm by looking beyond ferromagnets. Recent studies of relativistic magnetic and magnetotransport anisotropy effects, which in principle are equally well present in materials with ferromagnetically and antiferromagnetically ordered spins, have inspired our search for antiferromagnetic semiconductors suitable for high-temperature spintronics. Since these are not found among the magnetic counterparts of common III-V or II-VI semi- conductors, we turn the attention in this paper to high N eel temperature I-II-V magnetic compounds whose electronic structure has not been previously identified. Our combined experimental and theoretical work on LiMnAs provides basic prerequisite for the systematic research of this class of materials by demonstrating the feasibility to grow single crystals of group-I alkali metal compounds by molecular beam epitaxy, by demonstrating the semiconducting band structure of the I-Mn-Vs, and by analyzing their spin-orbit coupling characteristics favorable for spintronics.
We discuss the character of states near the Fermi level in Mn doped GaAs, as revealed by a survey of dc transport and optical studies over a wide range of Mn concentrations. A thermally activated valence band contribution to dc transport, a mid-infra
red peak at energy hbar omega approx 200 meV in the ac- conductivity, and the hot photoluminescence spectra indicate the presence of an impurity band in low doped (<<1% Mn) insulating GaAs:Mn materials. Consistent with the implications of this picture, both the impurity band ionization energy inferred from the dc transport and the position of the mid-infrared peak move to lower energies and the peak broadens with increasing Mn concentration. In metallic materials with > 2% doping, no traces of Mn-related activated contribution can be identified in dc-transport, suggesting that the impurity band has merged with the valence band. No discrepancies with this perception are found when analyzing optical measurements in the high-doped GaAs:Mn. A higher energy (hbar omega approx 250 meV) mid-infrared feature which appears in the metallic samples is associated with inter-valence band transitions. Its red-shift with increased doping can be interpreted as a consequence of increased screening which narrows the localized-state valence-band tails and weakens higher energy transition amplitudes. Our examination of the dc and ac transport characteristics of GaAs:Mn is accompanied by comparisons with its shallow acceptor counterparts, confirming the disordered valence band picture of high-doped metallic GaAs:Mn material.
